Apparatus for contact reaction between different gases

ABSTRACT

An apparatus for contact reaction between different gases, which apparatus contains:  
     a hollow body consisting of a first feeding section and a second feeding section,  
     said first feeding section to be fed with a first reactive gas being made of a porous material having through-pores, and  
     said second feeding section to be fed with a second reactive gas being formed so as to surround the first feeding section, thereby the first reactive gas being successively diffused toward the second feeding section from the through-pore ends to give rise to a contact reaction between the first reactive gas and the second reactive gas through the through-pores of the first feeding section, and in which apparatus  
     the total areas of the openings of the through-pore ends which are present on an outer surface of the first feeding section being faced to an internal surface of the second feeding section of the first feeding section has an area sufficient to be an amount capable of matching an amount of the second reactive gas fed, and  
     each of the opening areas of said through-pore ends has an area sufficient to show a linear velocity of diffusion of the first reactive gas at said through-pore ends in a through-pore axial direction larger than a linear velocity of diffusion of the second reactive gas at said through-pore ends in a through-pore axial direction opposite to the direction of diffusion of the first reactive gas. The apparatus can specify and control the feeding conditions of different reactive gases comprehensively and appropriately, enabling uniform contact and reaction of the gases and giving improved productivity.

BACKGROUND OF THE INVENTION

[0001] (1) Field of the Invention

[0002] The present invention relates to an apparatus for contact reaction between different gases. More particularly, the present invention relates to an apparatus for contact reaction between different gases which can specify and control the feeding conditions of different reactive gases comprehensively and appropriately, can give rise to uniform contact and reaction of the gases and can give improved productivity.

[0003] (2) Description of Related Art

[0004] As a contact reaction between different gases, there is known, for example, a partial oxidation reaction which comprises subjecting a hydrocarbon gas (e.g. methane or a naphtha) to a contact reaction with oxygen or air to produce a synthetic gas composed of carbon monoxide and hydrogen. In this partial oxidation reaction, it is necessary for higher productivity to control the amount of oxygen or air fed, at a level matching the amount of the hydrocarbon gas fed. When the amount of oxygen or air fed is too large, oxidation proceeds more than necessary and the reaction product becomes carbon dioxide and water, making it impossible to obtain an intended synthetic gas. When the amount is too small, the reaction is insufficient, making it impossible to obtain an intended gas efficiently.

[0005] In such a partial oxidation reaction, there is used an apparatus having an oxygen- or air-feeding section made of a porous material having though-pores so that oxygen or air can be fed to the reaction system in a uniformly dispersed state (Proceedings of the Fifth International Conference on Inorganic Membranes, Nagoya, Jun. 22-26, 1998, B-408, P-231).

[0006] In the above apparatus, it is possible to make fairly constant the amount of oxygen or air fed to the reaction system. With the apparatus, however, no comprehensive and reliable techniques have been established yet on (1) appropriate control of the amount of fed oxygen or air so as to match the amount of fed hydrocarbon gas, (2) prevention of counter-diffusion of hydrocarbon gas into the through-pores of the feeding section of oxygen or air, and (3) reduction of the pressure loss in the feeding section of oxygen or air.

SUMMARY OF THE INVENTION

[0007] In view of the above problems of the prior art, the present invention aims at providing an apparatus for contact reaction between different gases which can specify and control the feeding conditions of different reactive gases comprehensively and appropriately, can give rise to uniform contact and reaction of the gases and can give improved productivity.

[0008] The present inventor made a study in order to solve the above problems. As a result, the present inventor found out that the above aim could be achieved by setting the total of the opening areas of the through-pore ends present on the surface of the oxygen- or air-feeding section made of a porous material having through-pores, so that the amount of oxygen or air fed can match the amount of hydrocarbon gas fed and further by setting the opening area of each through-pore end so that the linear velocity of diffusion of oxygen or air in the through-pore can be at a particular level. The present invention has been completed based on the finding.

[0009] The present invention provides the following apparatus for contact reaction between different gases.

[0010] An apparatus for contact reaction between different gases, which apparatus comprises:

[0011] a hollow body consisting of a first feeding section and a second feeding section,

[0012] said first feeding section to be fed with a first reactive gas being made of a porous material having through-pores, and

[0013] said second feeding section to be fed with a second reactive gas being formed so as to surround the first feeding section, thereby the first reactive gas being successively diffused toward the second feeding section from the through-pore ends to give rise to a contact reaction between the first reactive gas and the second reactive gas through the through-pores of the first feeding section, and in which apparatus

[0014] the total areas of the openings of the through-pore ends which are present on an outer surface of the first feeding section being faced to an internal surface of the second feeding section of the first feeding section has an area sufficient to be an amount capable of matching an amount of the second reactive gas fed, and

[0015] each of the opening areas of said through-pore ends has an area sufficient to show a linear velocity of diffusion of the first reactive gas at said through-pore ends in a through-pore axial direction larger than a linear velocity of diffusion of the second reactive gas at said through-pore ends in a through-pore axial direction opposite to the direction of diffusion of the first reactive gas.

[0016] Furthermore, there are provided the following apparatuses usable for contact reaction between different gases:

[0017] an apparatus for contact reaction between different gases, wherein the first feeding section has a porosity of 1 to 50%,

[0018] an apparatus for contact reaction between different gases, wherein said total areas of the openings of the through-pore ends are sufficient to make a linear velocity of diffusion of the first reactive gas at the through-pore ends in a through-pore axial direction at least equal to a value of 0.3 to 1.4 cm/sec,

[0019] an apparatus for contact reaction between different gases, wherein the total pressure loss in the through-pores of the first feeding section is 3 atm or less,

[0020] an apparatus for contact reaction between different gases, wherein the first reactive gas is oxygen or air and the second reactive gas is a hydrocarbon, and

[0021] an apparatus for contact reaction between different gases, wherein the first feeding section has a cylindrical shape.

BRIEF DESCRIPTION OF THE DRAWINGS

[0022]FIG. 1 is a drawing schematically showing an embodiment of the apparatus for contact reaction between different gases according to the present invention.

[0023]FIG. 2 is a drawing schematically showing a first feeding section made of a porous material having through-pores, which is a constituent of the apparatus of FIG. 1.

DESCRIPTION OF PREFERRED EMBODIMENT

[0024] The embodiment of the apparatus of the present invention is specifically described below with referring to the accompanying drawings.

[0025] As shown in FIG. 1, the apparatus 10 of the present invention for contact reaction between different gases is an apparatus for subjecting different reactive gases to a contact reaction and has:

[0026] a first feeding section 2 having a hollow tubular shape being made of porous material and having through-pores perpendicular to the axis of the section, into which a first reactive gas 1 is to be introduced, and

[0027] a second feeding section 4 formed around the first feeding section 2 covering the whole outer surface of the first feeding section, into which a second reactive gas 3 is to be introduced.

[0028] As shown in FIG. 2, the apparatus 10 of the present invention is constituted so that the first reactive gas 1 can pass through the through-pores of the first feeding section 2 and be successively diffused toward the second feeding section 4 perpendicular to the axis of the first feeding section from the ends 5 of the through-pores to give rise to a contact reaction between the first reactive gas 1 and the second reactive gas 3.

[0029] In FIG. 2, the ends 5 of the through-pores, present on the inner surface of the first feeding section 2 are not shown.

[0030] Ordinarily, a catalyst 7 is filled between the second feeding section 4 and the first feeding section 2. The first reactive gas 1 is introduced into the first feeding section 2 from an inlet for the first reactive gas (not depicted), is successively diffused from its through-pore ends 5 toward the second feeding section 4, and is subjected to a contact reaction with the second reactive gas 3 fed from an inlet for the second reactive gas (not depicted) in the portion in which the catalyst 7 is filled.

[0031] In this case, it is possible that the catalyst 7 is filled in the first feeding section 2 and the first reactive gas 1 is introduced into the second feeding section 4, is successively diffused toward the first feeding section 2 from the ends 5 of its through-pores, and is subjected to a contact reaction with the second reactive gas 3 introduced into the first feeding section, in the portion in which the catalyst 7 is filled.

[0032] In the apparatus 10 of the present invention, the total areas of the openings of the through-pore ends 5 which are present on an outer surface of the first feeding section 2 being faced to an internal surface of the second feeding section of the first feeding section 2 has an area sufficient to be an amount capable of matching an amount of the second reactive gas 3 fed, and

[0033] each of the opening areas of said through-pore ends 5 has an area sufficient to show a linear velocity of diffusion of the first reactive gas at said through-pore ends 5 in a through-pore axial direction larger than a linear velocity of diffusion of the second reactive gas at said through-pore ends in a through-pore axial direction opposite to the direction of diffusion of the first reactive gas 1.

[0034] As to the apparatus for contact reaction between different gases, used in the present invention, there is no particular restriction as long as the apparatus can give rise to a contact reaction between different reactive gases. As the apparatus, there can be mentioned, for example, a partial oxidation reaction apparatus wherein a hydrocarbon gas (e.g. methane or a naphtha) is reacted with oxygen or air to produce a synthetic gas composed of carbon monoxide and hydrogen, an apparatus for selective oxidation of carbon monoxide, a dehydrogenation reaction apparatus wherein propane is reacted with oxygen or air to produce propylene, an oxidation reaction apparatus wherein butane is reacted with oxygen or air to produce maleic anhydride, and a partial oxidation reaction apparatus wherein methane is reacted with oxygen or air to produce acetaldehyde.

[0035] The reactive gases used in the present invention can be any reactive gases which react with each other when contacted. The present invention is particularly effective to gases which need be fed under appropriately specified and controlled conditions, for example, gases used in the above-mentioned partial oxidation reaction.

[0036] As specific combinations of the reactive gases used in the present invention, there can be mentioned, for example, a hydrocarbon gas (e.g. methane or a naphtha) and oxygen or air, propane and oxygen or air, carbon monoxide and oxygen or air, and butane and oxygen or air.

[0037] As to the first feeding section, there is no particular restriction as long as the first feeding section is made of a porous material having through-pores from the inner surface to the outer surface thereof. However, the first feeding section preferably has a cylindrical shape; as the material, there can be mentioned, for example, metal, alumina, titania, zirconia, cordierite, zeolite, silicon nitride, silicon carbide and mullite.

[0038] The porosity (as measured by the Archimedes method) of the through-pores of the first feeding section is specifically set preferably at 1 to 50%, more preferably at 5 to 30%, and more preferably at 10 to 20%. This porosity corresponds to [(opening areas (S) of individual through-pore ends)/(surface area of first feeding section)×100].

[0039] When the porosity of the through-pores of the first feeding section is less than 1%, a very large pressure difference is required in order to secure the necessary amount of air or oxygen fed. When the porosity is more than 50%, it may be difficult to secure the specified linear velocity of diffusion of the first reactive gas.

[0040] The linear velocity of diffusion of the first reactive gas at the through-pore ends in the perpendicular direction of the axis of the first gas feeding section is preferably specified so as to be at least equal to a value of 0.3 to 1.4 cm/sec. The reason for this requirement is given below.

[0041] As to the interdiffusion between two different gases when they are mixed, the following formula proposed by Fujita in the report under the title of [“Diffusion Coefficient in Gas Phase (Member s Contribution)”, Kagakukikai, Vol. 15, No. 5, 1951, pp. 234 to 236, contributed by Shigebumi Fujita].

D=0.00070T ^(1.833)(1/M ₁+1/M ₂)^(½)/{(Tc ₁ /Pc ₁)^(⅓)+(Tc ₂ /Pc ₂)^(⅓)}³  (1)

[0042] In the formula (1), D is an interdiffusion coefficient (cm²/sec), Tc is a critical temperature (K), Pc is a critical pressure (atm), T is a temperature (K), M is a molecular weight, and 1 and 2 in M₁, M₂, Tc₁, Pc₁, Tc₂, and Pc₂ are each the kind of a gas.

[0043] From the above formula, it is appreciated that the interdiffusion coefficient D is in a range of approximately 0.1 to 2 cm²/sec although it differs depending upon the kinds and temperatures of gases.

[0044] The linear velocity of diffusion of the second reactive gas depends upon the concentration gradient. When, for example, the concentration at the reaction side (the second feeding section) is 100% and the concentration at the first feeding section is 0%, the average diffusion distance x at t=1 second becomes 0.3 to 1.4 cm from x=(Dt)^(½).

[0045] Consequently, when the average linear velocity of diffusion of the second reactive gas in a through-pore axial direction is in a range of 0.3 to 1.4 cm/sec, it becomes necessary to set the linear velocity of diffusion of the first reactive gas at a level equal to or larger than the above linear velocity of diffusion of the second reactive gas, in a direction perpendicular to the axis of the first feeding section, that is, a through-pore axial direction opposite to the direction of diffusion of the second reactive gas, in order to prevent the counter-diffusion of the second reactive gas. Therefore, the linear velocity of diffusion of the first reactive gas at each through-pore end in the through-pore axial direction is preferably set so as to be at least equal to a value of 0.3 to 1.4 cm/sec.

[0046] If the linear velocity of diffusion of the first reactive gas at each through-pore end in a direction perpendicular to the axis of the first feeding section is too large, that is, the opening area of the end of each through-pore is too small, the pressure loss in the through-pores of the first feeding section increases and such an apparatus may be low in practical usability. Hence, the opening area of the end of each through-pore is sufficient to keep the pressure loss in the through-pores of the first feeding section preferably at 3 atm or less, more preferably at 1 atm or less.

[0047] The reason for the above setting is as follows. Use of a pressure lower than 10 atm is effective from the standpoints of law regulation and economy. A pressure loss exceeding 30% of 10 atm, i.e. 3 atm is very disadvantageous economically; therefore, a pressure loss of 10% (1 atm) or less is preferred.

[0048] Next, the following calculations were made for the preparation of an apparatus for selective oxidation of carbon monoxide, a reaction tube which comprises:

[0049] a stainless steel tube having an inner diameter of 25 mm,

[0050] a porous alumina tube inserted into the stainless steel tube, having an outer diameter of 17 mm and a thickness of 2.5 mm, and

[0051] a catalyst filled between the above two tubes, and whose reaction portion has an effective length of 200 mm, and passing, through the catalyst-filled portion, a reactive gas composed of 20% of hydrogen, 10% of water, 1,000 ppm of carbon monoxide and the remainder of nitrogen.

[0052] When the space velocity of the reactive gas is 80,000 h⁻¹, the velocity is calculated as follows.

((2.5×2.5−1.7×1.7)/4)×3.14×20×80,000=4,220,160 Nml/h=70.4 Nl/min

[0053] Meanwhile, the amount of carbon monoxide (1,000 ppm) fed is calculated as follows.

70,400×0.001=70.4 Nm1/min

[0054] The amount of oxygen required is equimolar to carbon monoxide, i.e. 70.4 Nml/min. This is because oxygen in an equimolar amount to that of carbon monoxide is required to attain the complete selective oxidation of carbon monoxide. The amount of air required is calculated as 5 times the amount of oxygen required, i.e. 352 Nml/min.

[0055] Since the surface area of the porous alumina is 1.7×3.14×20=106.8 cm², the required amount of air passing through the unit surface area of the porous alumina is calculated as in the following formula (2).

352/106.8=3.3 Nml/min·cm²   (2)

[0056] Meanwhile, the inter-diffusion coefficient of gases can be calculated from the above formula (1) (Fujita s formula).

[0057] Here, there is calculated an interdiffusion coefficient D between hydrogen (having the largest diffusion velocity) and oxygen, both of which are main components.

[0058] Calculation of the formula (1) is made by substituting T (temperature)=433 K (160° C.), M₁ (hydrogen mass)=2, M₂ (oxygen mass)=32, Tc₁ (critical temperature of hydrogen)=32.98 K, Pc₁ (critical pressure of hydrogen)=1.293 MPa=12.8 atm, Tc₂ (critical temperature of oxygen)=154.58 K, and Pc₂ (critical pressure of oxygen)=5.043 MPa=49.8 atm, whereby are obtained D=1.53 cm²/sec and average diffusion distance per second=(1.53×1)^(½)=1.24 cm/sec.

[0059] Therefore, in order to prevent the counter-diffusion of hydrogen gas into air side, the linear velocity of diffusion of oxygen is required to be 74.4 cm/min or more as shown in the following formula (3).

1.24 cm/sec=74.4 cm/min  (3)

[0060] In this respect, please note that the obtained linear diffusion velocity is one for the case of hydrogen gas having the largest linear velocity. Thus, the required linear velocity would become small in the case of the other reaction gas, such as hydrocarbon.

[0061] Then, the porosity of the first feeding section is calculated, by comparing an amount per unit area of air (2) to be required for the reaction with an amount per unit area of air (3) to be required for the prevention of hydrogen diffusion to the direction opposite to the follow of the air through the through-holes calculated from the diffision-velocity. That is, the porosity can be calculated from the above-mentioned formula (2)/the above-mentioned formula (3) and becomes 3.3/74.4×100=0.044×100=4.4%.

[0062] Thus, when a porous body having the porosity of 4.4% or less at the rate of 3.3 Nml/min cm² or more, the linear velocity of diffusion of oxygen becomes a desired level or more. However, since a smaller porosity gives a larger pressure loss, a large porosity is preferably used in designing. Hence, the porosity is most suitably 4.4%.

[0063] As described above, the present invention can provide an apparatus for contact reaction between different gases which can specify and control the feeding conditions of different reactive gases comprehensively and appropriately, can give rise to uniform contact and reaction of the gases and can give improved productivity. 

What is claimed is:
 1. An apparatus for contact reaction between different gases, which apparatus comprises: a hollow body consisting of a first feeding section and a second feeding section, said first feeding section to be fed with a first reactive gas being made of a porous material having through-pores, and said second feeding section to be fed with a second reactive gas being formed so as to surround the first feeding section, thereby the first reactive gas being successively diffused toward the second feeding section from the through-pore ends to give rise to a contact reaction between the first reactive gas and the second reactive gas through the through-pores of the first feeding section, and in which apparatus the total areas of the openings of the through-pore ends which are present on an outer surface of the first feeding section being faced to an internal surface of the second feeding section of the first feeding section has an area sufficient to be an amount capable of matching an amount of the second reactive gas fed, and each of the opening areas of said through-pore ends has an area sufficient to show a linear velocity of diffusion of the first reactive gas at said through-pore ends in a through-pore axial direction larger than a linear velocity of diffusion of the second reactive gas at said through-pore ends in a through-pore axial direction opposite to the direction of diffusion of the first reactive gas.
 2. An apparatus for contact reaction between different gases according to claim 1, wherein the first feeding section has a porosity of 1 to 50%.
 3. An apparatus for contact reaction between different gases according to claim 1 or 2, wherein said total areas of the openings of the through-pore ends are sufficient to make a linear velocity of diffusion of the first reactive gas at the through-pore ends in a through-pore axial direction at least equal to a value of 0.3 to 1.4 cm/sec.
 4. An apparatus for contact reaction between different gases according to claim 1, wherein the total pressure loss in the through-pores of the first feeding section is 3 atm or less.
 5. An apparatus for contact reaction between different gases according to claim 1, wherein the first reactive gas is oxygen or air and the second reactive gas is a hydrocarbon.
 6. An apparatus for contact reaction between different gases according to claim 1, wherein the first feeding section has a cylindrical shape. 